Research in the Waldie Group
Achieving a sustainable chemical future will require the development of efficient processes for the interconversion of electrical and chemical energy for renewable fuels production, fuel cell applications, and the synthesis of chemical feedstocks. The Waldie Group is interested in the rational design of molecular catalysts with targeted reactivity for these applications. We apply concepts from synthetic inorganic and organometallic chemistry coupled with electrochemical and spectroscopic techniques to prepare, understand, and optimize these systems and their reactivity.
Electro-Oxidation of Chemical Fuels
The electrochemical oxidation of fuels, such as H2, formic acid, and methanol, serves as the anodic half-reaction in fuel cells for electricity generation. Understanding how to promote these reactions through catalysis is critical to advance these technologies. We target molecular electrocatalysts that operate with high selectivity under mild conditions and offer precise active site control. Our efforts focus on earth abundant transition metal complexes with functional ligands to promote key proton & electron transfers.
Redox-Active Ligands as Electron Reservoirs
The redox activity of first-row transition metal ions is dominated by one-electron processes, but the introduction of redox-active ligands can be an effective strategy for achieving multielectron behavior. Our efforts focus on phenylenediamide complexes that exhibit a reversible two-electron oxidation. We use experimental & computational tools to study these systems, as well as to identify how their redox activity can be applied to promote small molecule activation via ligand-to-substrate electron transfer or hydrogen atom transfer.
Electrocatalytic Hydrogenation of Carbonyls
The electrification of organic synthesis offers several advantages over traditional chemical methods – for carbonyl reduction, this means replacing stoichiometric reducing agents or hydrogen gas with an electrode as the terminal reductant. By considering the thermodynamic requirements for carbonyl hydrogenation, we develop molecular electrocatalysts that operate under mild conditions in conjugation with acid co-catalysts to deliver a broad reactivity scope for sustainable organic synthesis.
